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To achieve the unlimited goal to tailor the structure\u2013activity relationship in multicomponent systems, entropy\u2010driven composition engineering presents substantial potential, by fabricating high\u2010entropy anion\u2010regulated transition metal compounds as sophisticated oxygen evolution reaction electrocatalysts. Herein, a versatile 2D high\u2010entropy metal phosphorus trisulfide is developed as a promising and adjustable platform. Leveraging the multiple electron couplings and d\u2013p orbital hybridizations induced by the cocktail effect, the exceptional oxygen evolution catalytic activity is disclosed upon van der Waals material (MnFeCoNiZn)PS\n                    <jats:sub>3<\/jats:sub>\n                    , exhibiting an impressively low overpotential of 240\u00a0mV at a current density of 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , a minimal Tafel slope of 32\u00a0mV dec\n                    <jats:sup>\u22121<\/jats:sup>\n                    , and negligible degradation under varying current densities for over 96 h. Density functional theory calculations further offer insights into the correlation between orbital hybridization and catalytic performance within high\u2010entropy systems, underscoring the contribution of active phosphorus centers on the substrate to performance enhancements. Moreover, by achieving electron redistribution to optimize the electron coordination environment, this work presents an effective strategy for advanced catalysts in energy\u2010related applications.\n                  <\/jats:p>","DOI":"10.1002\/adma.202404772","type":"journal-article","created":{"date-parts":[[2024,6,1]],"date-time":"2024-06-01T09:59:05Z","timestamp":1717235945000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":78,"title":["Augmented Electrochemical Oxygen Evolution by d\u2013p Orbital Electron Coupling"],"prefix":"10.1002","volume":"36","author":[{"given":"Ning","family":"Sun","sequence":"first","affiliation":[{"name":"State Key Laboratory of Information Photonics and Optical Communications School of Science Beijing University of Posts and Telecommunications  Beijing 100876 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhichuan","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Information Photonics and Optical Communications School of Science Beijing University of Posts and Telecommunications  Beijing 100876 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhuangzhuang","family":"Lai","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Green Chemistry Engineering and Industrial Catalysis Centre for Computational Chemistry and Research Institute of Industrial Catalysis School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai 200237 P. 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